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Krinner Et Al 02233 Nature.Pdf letters to nature Methods 23. Nørskov, J. K. et al. Universality in heterogeneous catalysis. J. Catal. 209, 275–278 (2002). 24. Da Silva, J. L. F., Stampfl, C. & Scheffler, M. Adsorption of Xe atoms on metal surfaces: new insights The growth experiments were carried out in a Philips CM300 FEG TEM equipped with an from first-principles calculations. Phys. Rev. Lett. 90, 066104 (2003). in situ cell13. This system provides images with a resolution better than 0.14 nm of samples 25. Vanderbilt, D. H. Soft self-consistent pseudopotentials in a generalized eigenvalue formalism. Phys. exposed to reactive gases and elevated temperatures. ATietz FastScan-F114 CCD was used Rev. B 41, 7892–7895 (1990). for recording TEM images. The image acquisition time was adjusted to suit the reshaping 21 26. Kresse, G. & Forthmu¨ller, J. Efficiency of ab-initio total energy calculations for metals and of the Ni nanocrystals and ranged from 2 to 10 frames s . A total of 16 video sequences semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6, 15–50 (1996). (each consisting of 300–1,200 consecutive high-resolution images) showing the coupling of graphene growth to Ni step-edge dynamics were recorded in six different growth experiments. The electron beam intensity was kept in the interval 0.2–2 A cm22, which was Supplementary Information accompanies the paper on www.nature.com/nature. sufficiently low to avoid any influence of the electron beam on the growth. Growth experiments with the electron beam switched off resulted in the same carbon nanofibre Acknowledgements We gratefully acknowledge the participation of the CTCI Foundation, structures as in the low-dose in situ experiments. Taiwan, in the establishment of the TEM facility at Haldor Topsøe A/S. S.H. acknowledges The self-consistent DFT calculations were performed using the LDA14 or the GGA- support from the Danish Research Council, STVF. F.A.P. and J.K.N. acknowledge computational RPBE approximation16 for exchange and correlation. The interaction of the graphene resources from the Danish Center for Scientific Computing. C.L.-C. acknowledges support from overlayer with the Ni(111) surface was dominated by van der Waals forces. The LDA for Facultad de Ciencias, Universidad de Ca´diz, Puerto Real, Spain, for a sabbatical visit to Haldor the exchange and correlation term is known to give the best description of such weak Topsøe A/S. interactions24. We have therefore used LDA for calculating the adsorption energy and diffusion energy barrier for C and Ni adatoms on the clean Ni(111) surface and the Competing interests statement The authors declare competing financial interests: details graphene–Ni(111) interface. The adsorption energies and diffusion energy barriers on the accompany the paper on www.nature.com/nature. clean Ni(111) surface calculated by the GGA-RPBE approximation were found to be essentially the same. However, within the GGA-RPBE approximation we found no Correspondence and requests for materials should be addressed to S.H. ([email protected]). adhesion of the graphene overlayer to the Ni(111) surface. The ionic cores are described by ultrasoft pseudopotentials25 and the one-electron valence states were expanded in a basis of plane waves with kinetic energy below 25 Ry. The electron density was determined self-consistently by iterative diagonalization of the Kohn–Sham hamiltonian, Pulay mixing26 of the resulting electronic density and Fermi occupation of the Kohn–Sham states (k BT ¼ 0.1 eV). All total energy calculations were .............................................................. extrapolated to zero electronic temperature and performed with the magnetic moment of the nickel surface taken into account. Enhanced ice sheet growth in Eurasia The Ni(111) surface was modelled by a periodic repetition of a three-layer slab, whereas a slab thickness of nine layers was used in the [211] direction to create a stepped surface and a thickness comparable to the Ni(111) surface. In both cases, the slabs were separated owing to adjacent ice-dammed lakes by ,10 A˚ of vacuum. In the Ni(111) model, the top layer was allowed to fully relax, whereas in the Ni(211) model, the uppermost close-packed (111) layer was relaxed fully. G. Krinner1, J. Mangerud2, M. Jakobsson3, M. Crucifix4*, C. Ritz1 The remaining layers were kept fixed in the bulk geometry with a calculated equilibrium & J. I. Svendsen2 lattice constant of 3.52 A˚ . For all calculations on Ni(111), a p(2 £ 2) lateral unit cell was used, giving C and Ni adsorbate coverages of 0.25 ML, whereas the C/Ni ratio for the 1LGGE, CNRS-UJF Grenoble, BP 96, F-38402 Saint Martin d’He`res, France graphene overlayer was 2. For the Ni(211) surface, a (1 £ 2) unit cell was used in the 2 calculations with a one-to-one coverage of adsorbate to Ni step edge atoms. A sampling of Department of Earth Science, University of Bergen, and Bjerknes Centre for 4 £ 4 £ 1 Monkhorst–Pack special k-points was used, resulting in 8 k-points in the Climate Research, Alle´gt. 41, N-5007 Bergen, Norway 3 irreducible Brillouin zone. Center for Coastal and Ocean Mapping/Joint Hydrographic Center, Chase Ocean Engineering Laboratory, 24 Colovos Road, Durham, New Hampshire 03824, Received 20 August; accepted 5 December 2003; doi:10.1038/nature02278. USA 1. Baughman, R. H., Zakhidov, A. A. & de Heer, W. A. Carbon nanotubes—the route towards 4Institut d’Astronomie et de Ge´ophysique G. Lemaıˆtre, Universite´ catholique de applications. Science 297, 787–792 (2002). Louvain, chemin du Cyclotron, 2, B-1348 Louvain-la-Neuve, Belgium 2. Ajayan, P. M. Nanotubes from carbon. Chem. Rev. 99, 1787–1799 (1999). 3. Rostrup-Nielsen, J. R., Sehested, J. & Nørskov, J. K. Hydrogen and synthesis gas by steam and CO2 * Present address: Met Office, Hadley Centre for Climate Prediction and Research, Fitzroy Road, Exeter reforming. Adv. Catal. 47, 65–138 (2002). EX1 3PB, UK 4. Ebbesen, T. W. & Ajayan, P. M. Large-scale synthesis of carbon nanotubes. Nature 358, 220–222 ............................................................................................................................................................................. (1992). Large proglacial lakes cool regional summer climate because of 5. Thess, A. et al. Crystalline ropes of metallic carbon nanotubes. Science 273, 483–487 (1996). their large heat capacity, and have been shown to modify 6. Kong, J., Soh, H. T., Cassell, A. M., Quate, C. F. & Dai, H. Synthesis of individual single-walled carbon nanotubes on patterned silicon wafers. Nature 395, 878–881 (1998). precipitation through mesoscale atmospheric feedbacks, as in 1 7. Boskovic, B. O. et al. Large-area synthesis of carbon nanofibres at room temperature. Nature Mater. 1, the case of Lake Agassiz . Several large ice-dammed lakes, with a 165–168 (2002). combined area twice that of the Caspian Sea, were formed in 8. Baker, R. T. K., Harris, P. S., Thomas, R. B. & Waite, R. J. Nucleation and growth of carbon deposits northern Eurasia about 90,000 years ago, during the last glacial from the nickel catalyzed decomposition of acetylene. J. Catal. 26, 51–62 (1972). 2 9. Rostrup-Nielsen, J. R. Equilibria of decomposition reactions of carbon monoxide and methane over period when an ice sheet centred over the Barents and Kara seas nickel catalysts. J. Catal. 27, 343–356 (1972). blocked the large northbound Russian rivers3. Here we present 10. Charlier, J.-C. & Iijima, S. in Growth Mechanisms of Carbon Nanotubes (eds Dresselhaus, M. S., high-resolution simulations with an atmospheric general circu- Dresselhaus, G. & Avouris, Ph.) Vol. 80, Topics in Applied Physics 55–80 (Springer, Heidelberg, 2001). 11. Clausen, B. S., Topsøe, H. & Frahm, R. Application of combined X-ray diffraction and absorption lation model that explicitly simulates the surface mass balance of techniques for in situ catalyst characterisation. Adv. Catal. 42, 315–344 (1998). the ice sheet. We show that the main influence of the Eurasian 12. Topsøe, H. In situ characterisation of catalysts. Stud. Surf. Sci. Catal. 130, 1–21 (2000). proglacial lakes was a significant reduction of ice sheet melting at 13. Hansen, P. L. et al. Atom-resolved imaging of dynamic shape changes in supported copper the southern margin of the Barents–Kara ice sheet through nanocrystals. Science 295, 2053–2055 (2002). 14. Jones, R. O. & Gunnarsson, O. The density functional formalism, its applications and prospects. Rev. strong regional summer cooling over large parts of Russia. In Mod. Phys. 61, 689–746 (1989). our simulations, the summer melt reduction clearly outweighs 15. Rosei, R. et al. Structure of graphitic carbon on Ni(111): A surface extended-energy-loss fine-structure lake-induced decreases in moisture and hence snowfall, such as study. Phys. Rev. B 28, 1161–1164 (1983). has been reported earlier for Lake Agassiz1. We conclude that the 16. Hammer, B., Hansen, L. B. & Nørskov, J. K. Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals. Phys. Rev. B 59, 7413–7421 (1999). summer cooling mechanism from proglacial lakes accelerated ice 17. Bengaard, H. S. et al. Steam reforming and graphite formation in Ni catalysts. J. Catal. 209, 365–384 sheet growth and delayed ice sheet decay in Eurasia and probably (2002). also in North America. 18. Trimm, D. L. The formation and removal of coke from nickel catalyst. Catal. Rev. Sci. Eng. 16, 155–189 We used the LMDZ3 (Laboratoire de Me´te´orologie Dynamique, (1977). 19. Alstrup, I. A new model explaining carbon filament growth on nickel, iron and Ni-Cu alloy catalysts. CNRS Paris) stretched-grid atmosphere general circulation model J. Catal. 109, 241–251 (1988). (AGCM). In addition to a present-day reference simulation (called 20. Rostrup-Nielsen, J. R. & Trimm, D. L. Mechanisms of carbon formation on nickel-containing ‘PD’), two simulations for 90 kyr before present (BP) were carried catalysts.
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